The two major challenges in industrial enzymatic catalysis are the limited number of chemical reaction types that are catalyzed by enzymes and the instability of enzymes under harsh conditions in industrial catalysis....The two major challenges in industrial enzymatic catalysis are the limited number of chemical reaction types that are catalyzed by enzymes and the instability of enzymes under harsh conditions in industrial catalysis.Expanding enzyme catalysis to a larger substrate scope and greater variety of chemical reactions and tuning the microenvironment surrounding enzyme molecules to achieve high enzyme performance are urgently needed.In this account,we focus on our efforts using the de novo approach to synthesis hybrid enzyme catalysts that can address these two challenges and the structure-function relationship is discussed to reveal the principles of designing hybrid enzyme catalysts.We hope that this account will promote further efforts toward fundamental research and wide applications of designed enzyme hybrid catalysts for expanding biocatalysis.展开更多
Electrochemical CO_(2)reduction to formate is a promising approach to store renewable electricity and utilize CO_(2).Tin oxide catalysts are efficient catalysts for this process,while the mechanisms underneath,especia...Electrochemical CO_(2)reduction to formate is a promising approach to store renewable electricity and utilize CO_(2).Tin oxide catalysts are efficient catalysts for this process,while the mechanisms underneath,especially the existence and role of oxidized tin species under CO2 electroreduction conditions remain unclear.In this work,we provide strong evidence on the presence of oxidized tin species on both SnO_(2)and Sn during CO_(2)reduction via in situ surface‐enhanced Raman spectroscopy,while in different nature.Reactivity measurements show similar activity and selectivity to formate production on SnO_(2)and Sn catalysts.Combined analysis of Raman spectra and reactivity results suggests that Sn(IV)and Sn(II)oxide species are unlikely the catalytic species in CO_(2)electroreduction to formate.展开更多
文摘The two major challenges in industrial enzymatic catalysis are the limited number of chemical reaction types that are catalyzed by enzymes and the instability of enzymes under harsh conditions in industrial catalysis.Expanding enzyme catalysis to a larger substrate scope and greater variety of chemical reactions and tuning the microenvironment surrounding enzyme molecules to achieve high enzyme performance are urgently needed.In this account,we focus on our efforts using the de novo approach to synthesis hybrid enzyme catalysts that can address these two challenges and the structure-function relationship is discussed to reveal the principles of designing hybrid enzyme catalysts.We hope that this account will promote further efforts toward fundamental research and wide applications of designed enzyme hybrid catalysts for expanding biocatalysis.
文摘Electrochemical CO_(2)reduction to formate is a promising approach to store renewable electricity and utilize CO_(2).Tin oxide catalysts are efficient catalysts for this process,while the mechanisms underneath,especially the existence and role of oxidized tin species under CO2 electroreduction conditions remain unclear.In this work,we provide strong evidence on the presence of oxidized tin species on both SnO_(2)and Sn during CO_(2)reduction via in situ surface‐enhanced Raman spectroscopy,while in different nature.Reactivity measurements show similar activity and selectivity to formate production on SnO_(2)and Sn catalysts.Combined analysis of Raman spectra and reactivity results suggests that Sn(IV)and Sn(II)oxide species are unlikely the catalytic species in CO_(2)electroreduction to formate.
